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<p>Selective oxidation of C-H bonds represents a pivotal transformation for upgrading hydrocarbon feedstocks into value-added chemicals, yet achieving this under mild conditions remains a formidable challenge. We herein disclose a single-atom photocatalytic system featuring nonsymmetric Fe-N<sub>3</sub>Br sites anchored on melem that enables efficient photooxidation of C(<i>sp</i><sup>3</sup>)-H bonds under mild conditions. The coordination environment facilitates Griffiths-type O<sub>2</sub> adsorption and realizes a high toluene conversion rate of 9.27 × 10<sup>4</sup> μmol g<sup>−1</sup> h<sup>−1</sup>. Experimental and theoretical studies indicate that the Fe-N<sub>3</sub>Br configuration reduces the Fe 3<i>d</i> splitting energy, enhances the O<sub>2</sub> adsorption, and facilitates O<sub>2</sub> activation, thereby promoting superoxide radical (•O<sub>2</sub><sup>-</sup>) generation. The catalyst demonstrates broad functional group tolerance (43 examples, up to 97% yield), and good scalability, enabling a 1000 mmol-scale continuous-flow reaction. This work demonstrates the importance of the single-atom site coordination in governing oxygen activation and provides a scalable, green photocatalytic platform for C-H functionalization.</p>

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Atomically dispersed iron on carbon nitride with enhanced oxygen adsorption for efficient and scalable photooxidation

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年5月29日

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  • Zhen Su,
  • Hua Long,
  • Siyi Song,
  • Rui-Rui Zhao,
  • Liang Zhou,
  • Ang Gao,
  • Ke Gao,
  • Wen-Jing Xiao

摘要

Selective oxidation of C-H bonds represents a pivotal transformation for upgrading hydrocarbon feedstocks into value-added chemicals, yet achieving this under mild conditions remains a formidable challenge. We herein disclose a single-atom photocatalytic system featuring nonsymmetric Fe-N3Br sites anchored on melem that enables efficient photooxidation of C(sp3)-H bonds under mild conditions. The coordination environment facilitates Griffiths-type O2 adsorption and realizes a high toluene conversion rate of 9.27 × 104 μmol g−1 h−1. Experimental and theoretical studies indicate that the Fe-N3Br configuration reduces the Fe 3d splitting energy, enhances the O2 adsorption, and facilitates O2 activation, thereby promoting superoxide radical (•O2-) generation. The catalyst demonstrates broad functional group tolerance (43 examples, up to 97% yield), and good scalability, enabling a 1000 mmol-scale continuous-flow reaction. This work demonstrates the importance of the single-atom site coordination in governing oxygen activation and provides a scalable, green photocatalytic platform for C-H functionalization.